This invention relates to a series of castable aluminum alloys with excellent creep and aging resistance, high electrical conductivity and thermal conductivity at elevated temperatures. The cast article comprises 0.4 to 2% by weight iron, 0 to 4% by weight nickel, 0.1 to 0.6 or about 0.1 to 0.8% by weight zirconium, optional 0.1 to 0.6% by weight vanadium, optional 0.1 to 2% by weight titanium, at least one inoculant such as 0.07-0.15% by weight tin, or 0.07-0.15% by weight indium, or 0.07-0.15% by weight antimony, or 0.02-0.2% by weight silicon, and aluminum as the remainder. The aluminum alloys contain a simultaneous dispersion of Al6Fe, Al3X (X=Fe, Ni) and/or Al9FeNi intermetallic in the eutectic regions and a dispersion of nano-precipitates of Al3ZrxVyTi1-x-y (0≤x≤1, 0≤y≤1 and 0≤x+y≤1) having L12 crystal structure in the aluminum matrix in between the eutectic regions. The processing condition for producing cast article of the present invention is disclosed in detail.
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1. An aluminum alloy comprising:
about 0.4 to 2% by weight iron;
0.25 to 0.8% by weight zirconium;
about 0.07 to 0.15% by weight tin, indium or antimony;
about 0.02 to 0.2% by weight silicon; and
aluminum as the remainder.
29. A method for manufacturing an aluminum alloy comprising the steps of casting an aluminum alloy mixture at about 750 to 950° C., the aluminum alloy mixture comprising:
about 0.4 to 2% by weight iron;
about 0.1 to 0.8% by weight zirconium;
about 0.07 to 0.15% by weight tin, indium or antimony;
about 0.02 to 0.2% by weight silicon;
an inoculant selected from the group consisting of Sn, In, Sb and their mixtures; and
aluminum as the remainder;
quenching the cast alloy after solidification; and
heat aging the cast article at a temperature in the range of about 300 to 450° C. for about 2 to 72 hours.
14. The aluminum alloy of
15. The aluminum alloy of
16. The aluminum alloy of
17. The aluminum alloy of
18. The aluminum alloy of
19. The aluminum alloy of
20. The aluminum alloy of
21. The aluminum alloy of
23. The aluminum alloy of
24. The aluminum alloy of
25. The aluminum alloy of
26. The aluminum alloy of
28. The cast aluminum article of
30. The method
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This application claims priority to and the benefit of and U.S. Provisional Application No. 62/129,311 entitled “High Temperature Creep Resistant Aluminum Superalloys,” filed Mar. 6, 2015, the disclosure of which is hereby incorporated by reference in its entirety.
The invention presented herein targets a new series of “aluminum superalloys” that are heat resistant and creep resistant at temperatures as high as 400° C. (752° F.) and that have high electrical conductivity and high thermal conductivity (at least 45% of annealed copper). The alloy can be fabricated through conventional casting method and is age-hardened and dispersion-hardened.
Aluminum alloys are one of the most common components of the light structures in aerospace, automotive, nuclear, and conductor wire and cable industry. However, in most cases, commercial aluminum alloys produced through conventional casting are not able to operate beyond 220° C. (428° F.). This is due to degradation of the microstructure by either dissolution or coarsening of the strengthening phase. Examples of such alloys include cast aluminum alloy 2xx.x, containing copper, 3xx.x, containing silicon and magnesium, and 7xx.x, containing zinc as the main alloying elements. Recent efforts have been made by researchers to produce aluminum alloys that contain scandium, which show improved mechanical properties at elevated temperatures. However, due to limited resources and production for scandium and very high cost of this element, the designed alloys have not found mass applications. Currently, traditional cast aluminum alloys are not capable of operating in applications such as automotive brake rotors, high power conductor wires and cables, engine components, and structural components in nuclear spent fuel storages, where good strength and high creep resistance are required at elevated temperatures as high as 400° C. (662° F.).
There have previously been attempts to produce aluminum alloys that can operate at elevated temperatures. The following patents represent some of these efforts:
J. A. Lee, “HIGH STRENGTH ALUMINUM ALLOY FOR HIGH TEMPERATURE APPLICATIONS” Patent No. U.S. Pat. No. 6,918,970, 2005.
D. Apelian. M. M. Makhlouf “ALUMINUM DIE CASTING ALLOY” Patent No. US 2013/0199680 AL, 2013.
C. S. Huskamp, C. Booth-Morrison, D. C. Dunand, D. N. Seidman, J. M. Boileau, B. Ghaffari, “ALUMINIUM ALLOY WITH ADDITIONS OF SCANDIUM, ZIRCONIUM AND ERBIUM” US 2013/0220497, filed 29 Aug. 2013.
Among these alloys, NASA series (U.S. Pat. No. 6,918,970) have found their way to industrial applications such as automotive engine components. These alloys are mainly improved 3xx.x cast aluminum alloys containing high Si content. Examples are NASA 358, 388 and 398, which comprise 6-25 wt. % Si and 5-8 wt. % Cu as the main alloying elements. The best performance NASA 398 alloy is claimed to be able to operate in the temperature range of 260-371° C. (500-700° F.).
From the preceding patent, it is realized that the high-temperature stability for these alloys originates from the presence of three different types of precipitates in the system namely Al2Cu (θ′), Al2CuMg (S′), and heat-resistant Al3X (X=Ti, V, Zr). The first two types are stabilized by: i) controlling the ratio of Cu/Mg in the alloy; and ii) simultaneous addition of transition metals such as Ti, V, and Zr. The patent states that its alloy shows good thermal stability at temperatures as high as 371° C. (700° F.). The published specifications on this material (NASA 398 alloy), however, show a very low thermal conductivity (120-130 W/m·K) in the temperature range of 25-371° C. (700° F.) and very low ductility (0.4% at 25° C. (77° F.) and 4.5% at 371° C. (700° F.)) which hinders its applications. Although these materials have excellent wear properties and high strength at room and elevated temperatures, they are not suitable for applications where high electrical and thermal conductivity and medium to high ductility are required. Such applications include: i) electricity and heat conductors in power transfer industry; ii) brake rotors and cylinder heads in automotive industry, and iii) interior compartments of the spent fuel storage canisters in nuclear industry.
Other production methods rather than traditional casting such as rapid solidification (RS) and powder metallurgy (PM) have also been utilized in producing aluminum alloys with outstanding properties at ambient and elevated temperatures. For example, Metamic-HT, an aluminum composite containing Al2O3 and B4C particles have outstanding mechanical properties and thermal conductivity at elevated temperatures as high as 350° C. (662° F.). However, the processing routes for such products are often very complicated and costly and cannot be scaled up for mass production.
Aluminum alloys are disclosed that have outstanding creep resistance, electrical conductivity and thermal conductivity at room temperature and elevated-temperatures. The alloys include about 0.4 to 2% by weight iron; about 0.1 to 0.8% by weight zirconium; about 0.07-0.15% by weight tin, indium or antimony; about 0.02-0.2% by weight silicon with aluminum as the remainder. Certain compositions can further include nickel at a concentration of up to about 4% by weight. Aluminum cast articles prepared from the disclosed aluminum alloys are also disclosed. In certain embodiments the alloys lack scandium.
In certain embodiments the aluminum alloy preferably include about 0.5 to 1.5% by weight iron and about 0.5 to 3.5% by weight nickel. Such alloys have superior electrical and thermal conductivity and better ductility while maintaining other superior properties.
In certain embodiments the aluminum alloy preferably include about 0.25 to 0.55% by weight zirconium. Such alloys can be prepared under casting conditions with moderate cooling rates after solidification.
In certain embodiments the aluminum alloy can include about 0.5 to 1.5% by weight iron, about 0.5 to 3.5% by weight nickel and about 0.25 to 0.55% by weight zirconium.
In certain embodiments the aluminum alloy preferably include about 0.27 to 0.42% by weight zirconium. Such alloys can be prepared under casting conditions with slow to moderate cooling rates after solidification.
In certain embodiments the aluminum alloy can include about 0.5 to 1.5% by weight iron, about 0.5 to 3.5% by weight nickel and about 0.27 to 0.42% by weight zirconium.
In certain embodiments the aluminum alloy can include about 0.5 to 1.5% by weight iron and about 1 to 3% by weight nickel.
In certain embodiments the aluminum alloy can include about 0.5 to 1.5% by weight iron, about 1 to 3% by weight nickel and about 0.25 to 0.55% by weight zirconium.
In certain embodiments the aluminum alloy can include about 0.5 to 1.5% by weight iron, about 1 to 3% by weight nickel and about 0.27 to 0.42% by weight zirconium.
In certain embodiments the aluminum alloy preferably includes about 0.82 to 1.22% by weight iron and about 1.65 to 2.35% by weight nickel. Such alloys provide superior thermal and electrical conductivities along with high ductility while maintaining other superior properties.
In certain embodiments the aluminum alloy can include about 0.82 to 1.22% by weight iron, about 1.65 to 2.35% by weight nickel and about 0.25 to 0.55% by weight zirconium.
In certain embodiments the aluminum alloy can include about 0.82 to 1.22% by weight iron, about 1.65 to 2.35% by weight nickel and about 0.27 to 0.42% by weight zirconium.
In certain embodiments the aluminum alloy can include nickel at a concentration of up to about 4% by weight and about 0.25 to 0.55% by weight zirconium.
In certain embodiments the aluminum alloy can include nickel at a concentration of up to about 4% by weight and about 0.27 to 0.42% by weight zirconium.
In certain embodiments the aluminum alloy can include about 0.1 to 0.6% by weight vanadium.
In certain embodiments the aluminum alloy can include about 0.1 to 2% by weight titanium.
In certain embodiments the aluminum alloy can include about 0.1 to 0.6% by weight vanadium and about 0.1 to 2% by weight titanium.
In certain embodiments the aluminum alloy can include a dispersion of intermetallic Al6Fe, Al3X (X=Fe, Ni) and Al9FeNi in intermetallic phases having an average diameter of about 200-600 nm.
In certain embodiments the aluminum alloy can include a dispersion of Al3ZrxVyTi1-x-y (0≤x≤1, 0≤y≤1 and 0≤x+y≤1) nano-precipitates, having the L12 crystal structure and an average diameter in the range of about 6-40 nm.
In certain embodiments the aluminum alloy can include nickel at a concentration of up to about 4% by weight and a dispersion of intermetallic Al6Fe and/or Al3Fe in intermetallic phases having an average diameter of about 200-600 nm.
In certain embodiments the aluminum alloy can include nickel at a concentration of up to about 4% by weight, a dispersion of intermetallic Al6Fe, Al3X (X=Fe, Ni) and Al9FeNi in intermetallic phases having an average diameter of about 200-600 nm, and a dispersion of Al3ZrxVyTi1-x-y (0≤x≤1, 0≤y≤1 and 0≤x+y≤1) nano-precipitates having L12 crystal structure and an average diameter in the range of about 6-40 nm.
In certain embodiments the aluminum alloy can include a dispersion of intermetallic Al6Fe and/or Al3Fe in intermetallic phases having an average diameter of about 200-600 nm and a dispersion of Al3ZrxVyTi1-x-y (0≤x≤1, 0≤y≤1 and 0≤x+y≤1) nano-precipitates having L12 crystal structure and an average diameter in the range of about 6-40 nm.
In certain embodiments the aluminum alloy can include filler materials or reinforcement materials selected from the group of materials consisting of silicon carbide (SiC), aluminum oxide (Al2O3), boron carbide (B4C), boron nitride (BN), titanium carbide (TiC), yttrium oxide (Y2O3), graphite, diamond particles, and their mixtures, the volume fraction of the filler materials comprising up to about 25% by volume of the metal matrix.
In certain embodiments the aluminum alloy can nickel at a concentration of up to about 4% by weight; filler materials or reinforcement materials selected from the group of materials consisting of silicon carbide (SiC), aluminum oxide (Al2O3), boron carbide (B4C), boron nitride (BN), titanium carbide (TiC), yttrium oxide (Y2O3), graphite, diamond particles, and their mixtures, the volume fraction of the filler materials comprising up to about 25% by volume.
In certain embodiments the aluminum alloy can be an aluminum cast article comprising a dispersion of intermetallic Al6Fe, Al3X (X=Fe, Ni) and Al9FeNi in intermetallic phases having an average size range of about 200-600 nm and a dispersion of Al3ZrxVyTi1-x-y (0≤x≤1, 0≤y≤1 and 0≤x+y≤1) nano-precipitates having L12 crystal structure and an average size range of about 6-40 nm.
Methods for manufacturing the aluminum metal matrix are also disclosed. The method includes casting at about 750 to 950° C. an alloy mixture of about 0.4 to 2% by weight iron; about 0.1 to 0.8% by weight zirconium; about 0.07-0.15% by weight tin, indium or antimony; about 0.02-0.2% by weight silicon, and an inoculant selected from the group of inoculants consisting of Sn, In, Sb and their mixtures; with aluminum as the remainder. The cast alloy can be quenched after solidification and can be aged at a temperature in the range of about 300 to 450° C. for about 2 to 72 hours.
In certain manufacturing methods aging can be at about 400 to 450° C. for about 24 to 72 hours.
In certain manufacturing methods the alloy mixture lacks scandium.
One embodiment of the present invention is an aluminum cast article with outstanding creep resistance, electrical conductivity and thermal conductivity at elevated temperatures. The cast article comprises:
Another embodiment of the present invention is a cast article with the aluminum alloy described above, further comprising a dispersion of intermetallic Al6Fe, Al3X (X=Fe, Ni) and Al9FeNi intermetallic phases with an average diameter in the range of about 200-600 nm.
Another embodiment of the present invention is a cast article with the aluminum alloy described above, comprising a dispersion of Al3ZrxVyTi1-x-y (0≤x≤1, 0≤y≤1 and 0≤x+y≤1) nano-precipitates, having L12 crystal structure with an average diameter range of about 6-20 or about 6-40 nm.
Another embodiment of the present invention is a cast article with the aluminum alloy described above, comprising about 0.4-2% by weight iron.
Another embodiment of the present invention is a cast article with the aluminum alloy described above, comprising about 0.5 to 4% by weight nickel.
Another embodiment of the present invention is a cast article with the aluminum alloy described above, comprising about 0.1 to 0.6% or about 0.1 to 0.8% by weight zirconium.
Another embodiment of the present invention is a cast article with the aluminum alloy described above, comprising about 0.07-0.15% by weight tin or about 0.07-0.15% by weight indium or about 0.07-0.15% by weight antimony.
Another embodiment of the present invention is a cast article with the aluminum alloy described above, comprising about 0.02-0.2% by weight silicon.
Another embodiment of the present invention is a cast article with the aluminum alloy described above, comprising about 0.1 to 0.6% by weight vanadium and about 0.1 to 2% by weight titanium.
Another embodiment of the present invention is a metal matrix having the composition
A series of heat resistant castable aluminum alloys with excellent creep and aging resistance and high electrical and thermal conductivity are disclosed. The outstanding creep resistance for these alloys results from: i) the presence of Al3ZrxVyTi1-x-y (0≤x≤1, 0≤y≤1 and 0≤x+y≤1) nano-precipitates with L12 crystal structure and the average diameter in the range of about 6-20 or about 6-40 nm, and ii) the reinforcement phase in the form of Al6Fe, Al3X (X=Ni, Fe) and Al9FeNi intermetallic precipitates with an average diameter in the range of about 200-600 nm. The average diameter of the reinforcement phase and nano-precipitates are measured via scanning electron microscopy (SEM) and atom probe tomography (APT) techniques, respectively. For SEM measurements, at least three images from three different regions are analyzed by means of common image analysis software to obtain the diameter of the captured intermetallic phase, and the average diameter is recorded for all captured intermetallics. For APT analysis, the obtained data is analyzed utilizing IVAS™ software to reconstruct the studied volume three-dimensionally that include nano-precipitates. The average diameter of the captured nano-precipitates is measured by the same software. The presence of Al3X (X=Fe, Ni) precipitates in the interdendritic regions and Al3ZrxVyTi1-x-y (0≤x≤1, 0≤y≤1 and 0≤x+y≤1) nano-precipitates in the dendritic regions creates a strong pinning force against dislocation motions at ambient and elevated temperatures. Since both hardening phases are thermally stable, the mechanical properties are maintained at elevated temperatures as high as 400° C. (752° F.).
The alloys disclosed herein are advantageous since they can be produced via low cost traditional casting method. In addition, utilizing low alloying element concentrations to produce these alloys allows superior electrical and thermal conductivity (at least 45% of annealed copper).
Another advantage is that these alloys are produced without using scandium as an alloying element, which results in a very low alloy cost.
The high number density of Al3ZrxVyTi1-x-y (0≤x≤1, 0≤y≤1 and 0≤x+y≤1) nano-precipitates, with the average diameter in the range of about 6-20 or about 6-40 nm, is produced by introducing an inoculant element into the alloy. The inoculant elements used in the invented alloys include Sn, In, and Sb. Thus the presence of the inoculant elements is important to obtain good strength and creep resistance at ambient and elevated temperatures.
The disclosed aluminum alloys provide light weight, low cost, highly electrically and thermally conductive, heat resistant, and creep resistant properties that are thermally stable in the temperature range of about 25-400° C. (about 77-752° F.).
These properties are achieved by aluminum alloys produced through traditional casting that contain:
The present invention comprises a series of aluminum alloys with combination of outstanding creep resistance and high electrical and thermal conductivity at ambient and elevated temperatures. The invented alloys are marked by an ability to perform in cast form, which is suitable for elevated temperatures. The high creep resistance of the invented alloys results from two main strengthening mechanisms: the intermetallic dispersion hardening and nano-precipitation hardening.
The intermetallic dispersion hardening relies on the formation of dispersed intermetallic phase in the interdendritic regions during solidification. In the present invention, about 0.4-2% by weight iron and about 0-4% by weight nickel is utilized to form a fine dispersion of Al6Fe, Al3X (X=Fe, Ni) and Al9FeNi intermetallic phases in the interdendritic regions. The volume fraction, shape, and diameter of Al3X (X=Fe, Ni) and Al9FeNi intermetallic phases depend on the concentration of Fe and Ni, the Fe/Ni concentration ratio, and the specific heat treatment conditions.
The nano-precipitation hardening relies on the formation of nano-precipitates in the aluminum matrix through specific heat treatment conditions. In the present invention, about 0.1 to 0.6 or about 0.1 to 0.8% by weight zirconium, about 0.1 to 0.6% by weight vanadium, and about 0.1-2% by weight titanium are used to create a high number density of coherent L12 Al3ZrxVyTi1-x-y (0≤x≤1, 0≤y≤1 and 0≤x+y≤1) nano-precipitates in the aluminum alloy. Since the atomic radius of vanadium (0.132 nm) is smaller than zirconium (0.159 nm) and titanium (0.176 nm), the lattice mismatch of the Al3ZrxVyTi1-x-y (0≤x≤1, 0≤y≤1 and 0≤x+y≤1) type precipitates can be reduced to closely match the lattice parameter of aluminum matrix. As a result, the coarsening resistance of the precipitates can be further increased by controlled addition of vanadium and titanium to zirconium-containing alloy. The volume fraction, diameter, and lattice mismatch of Al3ZrxVyTi1-x-y (0≤x≤1, 0≤y≤1 and 0≤x+y≤1) nano-precipitates depend on the concentration of Zr, V, and Ti, the corresponding Zr:V:Ti concentration ratio, and the specific heat treatment conditions.
The high creep resistance of the invented alloys relies on the presence of the heat resistant Al6Fe, Al3X (X=Fe, Ni), and Al9FeNi intermetallic phases and the heat resistant Al3ZrxVyTi1-x-y (0≤x≤1, 0≤y≤1 and 0≤x+y≤1) nano-precipitates. While the former contributes to strengthening of the interdendritic regions, the latter strengthens the dendritic regions. The strengtheners create barriers to dislocation glide and dislocation climb (i.e. the main creep mechanism) at elevated temperatures.
The specific concentration of alloying elements and heat treatment conditions are necessary to create the desired microstructure with desired diameter and volume fraction of both nickel-iron intermetallic phases and Al3ZrxVyTi1-x-y (0≤x≤1, 0≤y≤1 and 0≤x+y≤1) nano-precipitates.
Generally, the invented alloys after optimal processing contain about 0.3-0.8% by volume fraction Al3ZrxVyTi1-x-y (0≤x≤1, 0≤y≤1 and 0≤x+y≤1), and about 0-20% by volume fraction Al3X (X=Fe, Ni) and Al9FeNi.
In order to activate the strengtheners and achieve outstanding mechanical properties, the cast articles must have specific chemical compositions and heat treatments. These conditions are designed to maximize the strengthening effects through optimized formation of Al3ZrxVyTi1-x-y (0≤x≤1, 0≤y≤1 and 0≤x+y≤1), Al3X (X=Fe, Ni), and Al9FeNi phases.
The high-temperature strength is achieved in the present invention when using a T5 heat treatment consisting of aging at 400-450° C. (752-842° F.) for 24 to 72 hours. The unique composition and the corresponding heat treatment allow nearly full precipitation of Al3ZrxVyTi1-x-y (0≤x≤1, 0≤y≤1 and 0≤x+y≤1) nano-precipitates with high number density and average diameter in the range of 6-20 or 6-40 nm. Additionally, the fragmentation of the nickel-iron intermetallic phases during the heat treatment allows further improvement in ductility while maintaining the strength.
TABLE. 1
Thermal
Compressive
conductivity
Specs.
0.2% σY (MPa)
Strength (MPa)
(W/m · K)
Testing
RT
200° C.
300° C.
375° C.
RT
200° C.
300° C.
375° C.
RT
375° C.
temp.
Alloy
167
125
102
55
259
184
113
63
185
—
1 values in compressive mode
The aging-resistance of the present invention stems from the presence of heat resistant Al6Fe, Al3X (X=Fe, Ni) and Al9FeNi intermetallic phases, and Al3ZrxVyTi1-x-y (0≤x≤1, 0≤y≤1 and 0≤x+y≤1) nano-precipitates. The aging resistance is described as the retained room temperature strength after exposure to high temperature for several months.
The alloys produced according to the present invention are processed using traditional casting. The casting temperature is in the range of 750-950° C. (1382-1742° F.). The cast alloys are quenched in a quenching medium after solidification to maximize the content of solute atoms in the solid solution. This allows cooling rate that exceeds 10° C./s (50° F./s). The most preferred quenching medium is water at temperature between 25 to 40° C. (77 to 104° F.). After quenching, the cast article is aged at temperature in the range of 300 to 475° C. or 400 to 475° C. (572 to 887° F. or 752 to 842° F.) for 2 to 72 or 24 to 72 hours to achieve optimal properties.
The alloy of present invention may be heat treated in one or two-step aging processes. The two-step aging is performed on cast alloys to maximize room-temperature strength. While the first step aging at lower aging temperature creates a high number density of nuclei due to the higher chemical driving force, the second step aging at higher temperature accelerates the kinetics of precipitate growth to achieve optimal strength. For the one-step aging process, the cast article can be aged at temperature in the range of 350-475° C. for 2 to 72 to achieve optimal properties. For the two-step aging process, in the first step, the cast article can be aged at temperature in the range of 330-375° C. for 2 to 24 hours followed by the second step aging at 425-475° C. for 1 to 24 hours. The effect of two-step aging versus one-step aging is presented in
The alloy of the present invention can be used in either a bulk alloy form or as an alloy matrix for producing metal matrix composite (MMC). The metal matrix composite comprises the aluminum alloy of the present invention as the alloy matrix and filler materials in the form of particles, whiskers, chopped fibers, and continuous fibers. The MMC comprising the aluminum alloy of present invention and the filler materials can be produced by common techniques such as mechanically mixing and stirring the filler materials into the molten metal (that is compo-casting or stir-casting) or using ultrasonic waves to mix and distribute the filler materials into the molten metal.
The filler materials should not be confused with Al6Fe, Al3X (X=Fe, Ni) and Al9FeNi intermetallic phases or Al3ZrxVyTi1-x-y and (0≤x≤1, 0≤y≤1 and 0≤x+y≤1) nano-precipitates. The average diameter of the filler materials or the reinforcement material is typically in the 1-25 microns range. The filler materials or reinforcement materials include silicon carbide (SiC), aluminum oxide (Al2O3), boron carbide (B4C), boron nitride (BN), titanium carbide (TiC), yttrium oxide (Y2O3), graphite, diamond particles, and any combination of aforementioned particles. The volume fraction of the filler materials can vary up to 25% by volume.
The present invention has been described in detailed embodiments thereof. It is understood by those skilled in the art that modifications and variations in this detail may be made without departing from the spirit and scope of the claimed invention.
Vo, Nhon Q., Sanaty-Zadeh, Amirreza
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